Hydrogen storage and stability properties of Pd-Pt solid-solution nanoparticles revealed via atomic and electronic structure

Loku Singgappulige Rosantha Kumara, Osami Sakata, Hirokazu Kobayashi, Chulho Song, Shinji Kohara, Toshiaki Ina, Toshiki Yoshimoto, Satoru Yoshioka, Syo Matsumura, Hiroshi Kitagawa

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Abstract

Bimetallic Pd1-x Pt x solid-solution nanoparticles (NPs) display charging/discharging of hydrogen gas, which has relevance for fuel cell technologies; however, the constituent elements are immiscible in the bulk phase. We examined these material systems using high-energy synchrotron X-ray diffraction, X-ray absorption fine structure and hard X-ray photoelectron spectroscopy techniques. Recent studies have demonstrated the hydrogen storage properties and catalytic activities of Pd-Pt alloys; however, comprehensive details of their structural and electronic functionality at the atomic scale have yet to be reported. Three-dimensional atomic-scale structure results obtained from the pair distribution function (PDF) and reverse Monte Carlo (RMC) methods suggest the formation of a highly disordered structure with a high cavity-volume-fraction for low-Pt content NPs. The NP conduction band features, as extracted from X-ray absorption near-edge spectra at the Pd and Pt L III -edge, suggest that the Pd conduction band is filled by Pt valence electrons. This behaviour is consistent with observations of the hydrogen storage capacity of these NPs. The broadening of the valence band width and the down-shift of the d-band centre away from the Fermi level upon Pt substitution also provided evidence for enhanced stability of the hydride (ΔH) features of the Pd1-x Pt x solid-solution NPs with a Pt content of 8-21 atomic percent.

Original languageEnglish
Article number14606
JournalScientific reports
Volume7
Issue number1
DOIs
Publication statusPublished - Dec 1 2017

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atomic structure
solid solutions
electronic structure
nanoparticles
hydrogen
conduction bands
x rays
valence
fuel cells
hydrides
charging
Monte Carlo method
catalytic activity
synchrotrons
fine structure
distribution functions
photoelectron spectroscopy
substitutes
bandwidth
cavities

All Science Journal Classification (ASJC) codes

  • General

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Hydrogen storage and stability properties of Pd-Pt solid-solution nanoparticles revealed via atomic and electronic structure. / Kumara, Loku Singgappulige Rosantha; Sakata, Osami; Kobayashi, Hirokazu; Song, Chulho; Kohara, Shinji; Ina, Toshiaki; Yoshimoto, Toshiki; Yoshioka, Satoru; Matsumura, Syo; Kitagawa, Hiroshi.

In: Scientific reports, Vol. 7, No. 1, 14606, 01.12.2017.

Research output: Contribution to journalArticle

Kumara, Loku Singgappulige Rosantha ; Sakata, Osami ; Kobayashi, Hirokazu ; Song, Chulho ; Kohara, Shinji ; Ina, Toshiaki ; Yoshimoto, Toshiki ; Yoshioka, Satoru ; Matsumura, Syo ; Kitagawa, Hiroshi. / Hydrogen storage and stability properties of Pd-Pt solid-solution nanoparticles revealed via atomic and electronic structure. In: Scientific reports. 2017 ; Vol. 7, No. 1.
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